Coordination and activation of nitrous oxide by iron zeolites

Iron-containing zeolites are heterogeneous catalysts that exhibit remarkable activity in the selective oxidation of inert hydrocarbons and catalytic decomposition of nitrous oxide (N 2 O). The reduction of N 2 O is critical to both these functions, but experimental data tracking the iron active site...

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Vydané v:Nature catalysis Ročník 4; číslo 4; s. 332 - 340
Hlavní autori: Bols, Max L., Snyder, Benjamin E. R., Rhoda, Hannah M., Cnudde, Pieter, Fayad, Ghinwa, Schoonheydt, Robert A., Van Speybroeck, Veronique, Solomon, Edward I., Sels, Bert F.
Médium: Journal Article
Jazyk:English
Vydavateľské údaje: London Nature Publishing Group UK 01.04.2021
Nature Publishing Group
Springer Nature
Predmet:
639/638/440/950
639/638/563/979
639/638/77/884
639/638/77/885
639/638/77/887
Binding
Catalysis
Catalyst synthesis
Catalysts
Catalytic mechanisms
Chemistry
Chemistry and Materials Science
Decomposition
Density functional theory
Electronic structure
Fourier transforms
Heterogeneous catalysis
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Iron
Isomerization
Ligands
Low temperature
Nitrous oxide
Oxidation
Oxidizing agents
Reaction kinetics and dynamics
Spectrum analysis
Zeolites
ISSN:2520-1158, 2520-1158
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Shrnutí:Iron-containing zeolites are heterogeneous catalysts that exhibit remarkable activity in the selective oxidation of inert hydrocarbons and catalytic decomposition of nitrous oxide (N 2 O). The reduction of N 2 O is critical to both these functions, but experimental data tracking the iron active sites during N 2 O binding and activation are limited. Here, the N 2 O-ligated Fe( ii ) active site in iron-exchanged zeolite beta is isolated and characterized by variable-temperature Mössbauer, diffuse reflectance UV-vis-NIR and Fourier transform infrared spectroscopy. N 2 O binds through the terminal nitrogen atom with substantial backbonding from the Fe( ii ) centre at low temperature. At higher temperatures, the Fe–N 2 O interaction is weakened, facilitating isomerization to the O-bound form, which is competent in O-atom transfer. Density functional theory calculations show the geometric and electronic structure requirements for N 2 O binding and activation. A geometric distortion imposed by the zeolite lattice plays an important role in activating N 2 O. This highlights a mechanism for structural control over function in Fe-zeolite catalysts. Nitrous-oxide-mediated oxidation reactions can be effectively promoted by iron-containing zeolites, although structural information on the interaction between oxidant and metal centre is limited. Here, the authors report the characterization of the N 2 O-ligated Fe( ii ) active site in iron-exchanged zeolite beta.
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AC02-76SF00515; G0A2216N; V417018N; DGE-11474; CHE-1660611; 647755
National Science Foundation (NSF)
Flemish Science Foundation
USDOE Office of Science (SC), Basic Energy Sciences (BES)
National Science Foundation Graduate Research Fellowship Program
ISSN:2520-1158
2520-1158
DOI:10.1038/s41929-021-00602-4